Abstract The potassium aluminyl [K{Al(NONDipp)}]2 ([NONDipp]2?=[O{SiMe2NDipp}2]2?, Dipp=2,6‐iPr2C6H3) activates ethene towards carbonylation with CO under mild conditions. An isolated bis‐aluminacyclopropane compound reacted with CO via carbonylation of an Al?C bond, followed by an intramolecular hydrogen shift to form K2[Al(NONDipp)(μ‐CH2CH=CO‐1κ2C1,3‐2κO)Al(NONDipp)Et]. Restricting the chemistry to a mono‐aluminium system allowed isolation of [Al(NONDipp)(CH2CH2CO‐κ2C1,3)]?, which undergoes thermal isomerisation to form the [Al(NONDipp)(CH2CH=CHO‐κ2C,O)]? anion. DFT calculations highlight the stabilising influence of incorporated benzene at multiple steps in the reaction pathways.
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